Advice Please on a 5 Day Trip

Do you have the Rick Steves Switzerland book? If not, get it. It will help you immensely with your planning, and when they actually take the trip, give it to them to take with them.

If I had 4 nights in Switzerland (and it's always easiest to think nights, not days) in mid-September and such an early departure, I'd spend the first three in the Berner Oberland, the last day in Luzern, and the last night before the flight in Zurich.

Sunday: arrive in Zurich, take train right from airport to Lauterbrunnen. Sleep in Lauterbrunnen (3 nights). If they are early enough and have enough energy, they can take a lift to Mürren, Gimmelwald, or Allmendhubel and walk around (again, details in Rick's book). If they are tired, they can just walk the valley floor and take the bus back to Lauterbrunnen.
Monday and Tuesday: See the various sights in the Berner Oberland, including the Schilthornbahn and Piz Gloria. That's the place with the 007 exhibit; they shot a lot of On Her Majesty's Secret Service up there, and there is an extensive exhibit on the making of the movie. They can also walk the valley floor, take the train up to Jungfraujoch, see the Trummelbach Falls, and lots of other great stuff. Two full days isn't much time here, but it should give them a shot at a good weather day (the Schilthornbahn is expensive and the Jungfraujoch is very expensive, even with a Swiss Pass, so they're not worth doing in cloudy weather).
Wednesday: train to Luzern. Walk around this very pretty, "very Swiss" town, and maybe take a trip on the lake. By all accounts, Luzern is nicer than Zurich (literally - I have yet to see anyone who preferred Zurich!). Late train to Zurich to sleep there.
Thursday: Train to airport for flight home.

For a 7 AM flight, they probably don't want to spend the night before in Luzern; it's only a 70 minute train ride and the train goes right into the airport, but they'd have to be up even earlier than if they stay in Zurich!

Unfortunately, with such a short trip, she doesn't have time for scenic trains or for more than one alpine locale (and the Matterhorn is farther from Zurich than the Berner Oberland - and with no James Bond connection!). Remember that mountain weather is both unpredictable and rapidly changeable. You want to maximize time at one mountain locale, so you have a higher likelihood of at least one good weather day.

It's a surprise, so I can't ask her directly...

Wonderful gift idea! They both have passports valid through year-end 2017, right? If not, you may have to alter the surprise a tad to accommodate the paperwork.

Good catch by FastEddie! If they don't have passports, you want to get started on this now, to avoid having to pay extra for expediting. If they've never had a passport before, it can take some time to get the necessary documents (if their most recent one is not more than 5 years expired, it's a renewal rather than a new application, and so is easier and faster).

If they need passports, go directly to the official US State Department website https://travel.state.gov/content/passports/en/passports.html, and follow the steps. It will not only tell you everything you need to do, but also fill out the forms so you can just print them out.

With only 4 nights, I would spend 3 nights in Luzern, and the last night in Zurich, due to the early departure. There are many fun attractions in Luzern, most covered by the Swiss Pass. For active people, Mt. Pilatus and Mt. Rigi offer great views and walks, and are also covered by the Swiss Pass.

From Luzern, they can easily daytrip to Interlaken via the scenic train. Near Interlaken, they could visit castle Thun and Beatus caves, the open air Ballenberg musuem, and/or do some of these walks: http://www.backpackers.com.tw/forum/attachment.php?attachmentid=1988432&d=1482941572

I would skip the 007 museum. It would take them several hours to get up to the Schilthorn from Interlaken (train to Lauterbrunnen, cable car to Grutschalp, train or walk to Murren, 2 cable cars from Murren). I was there last week, and the 007 museum was extremely underwhelming. They don't have any movie artifacts, and the "interactive exhibits" are really lame. The view is nice, but only if the weather is great. They can see great views from the Luzern mountains with much less time and money invested. Also, both cable cars up to the Schilthorn were packed full, standing room only, jammed in with 99 other tourists. Just not worth it, IMHO.

I have to respectfully disagree with the comment that it will take several hours to get to Schilthorn from Interlaken. Searching a random weekday it looks like one way will take 1.5 hours. Train to Lauterbrunnen, bus to Stechelberg and lifts all the way up. Bus is timed to meet the train and lifts are fairly closely coordinated timewise.

http://fahrplan.sbb.ch/bin/query.exe/en?ld=std4.a&OK#focus

I've been to Luzern but not up to Mt. Rigi or Pilatus. I would make the trek up to the Schilthorn, it's a fabulous view weather permitting.

As far as Bond world, yes it's not for everyone. Most of us on the RS tour found it fun.

Harold's advice is spot on! The Lauterbrunnen Valley is far more scenic and emblematic of what she has seen on Rick's shows than Luzern is.

Thank you all for your feedback! My parents just got back from their trip, and they really enjoyed it thanks to all of your advice. I really appreciate it, and hope that someone else finds this useful in the future as well :)

I'm so glad they enjoyed their trip. Where did they end up staying - Luzern, Lauterbrunnen, or somewhere else?

So we took a lot of your advice, but they like to get a lot done in a few days. So I sent them to explore Lucern for the day, and sleep two nights in Interlaken. I then sent them for a day/night to Zermatt and finally had them take the Glacier Express around the rest of Switzerland and fly out. They really enjoyed their time!