Barcelona extra time

Not sure what's to see in Poblenou (it's the newer part of town) from a tourist perspective, Raval is a rough neighborhood that I'd stay away from, El Born is nice enough on foot. You could also consider exploring Gràcia, my favorite neighborhood of Barcelona. I would not bike within Barcelona, especially if you are new to the city, drivers can be quite aggressive.

There are other locations that I'd recommend around the city that maybe the tour does not cover like the Hospital Sant Pau, a Gaudi-esque modernisme complex built in the early 20th century. It has been named a UNESCO World Heritage Site and has significantly less tourists than the Sagrada Familia, although being only a 15 min walk from it,

Also one nice place that (surprisingly) has very few tourists is Parc del Laberint d'Horta I personally like it better than Park Güell. The park is one of the oldest in Barcelona and comprises a fantastic 18th-century neoclassical garden with the centerpiece of a labyrinth made up of trimmed cypress trees. I used to go there a lot when I was younger.

Both Montserrat and Girona (which is certainly not a village) can be easily done on your own using public transportation.

.... Anyone done Montserrat on their own, per the RS book..... Sure, it is easy. Just follow the book.

We did Monserrat on our own. Its very easy and I recommend you do that. For us, visiting Monserrat on our own by train and seeing the sites and hiking some of the trails was a whole day trip. So don't try to do it in a half day.
We took the 9:00 am (appx) train from Place Espanya (route R5) and got off at the second Monisterol stop to board the Cremallera (the railway,) which takes you up to the monastery. The train ride takes about an hour. You could also take the aerial cable car instead of the train, but that's a separate ticket, so you need to decide in advance which one you want to do.
The sites at the Monastery in one area. You won't get lost. We didn't think a personal guide would be worth it at Monserrat. But that's up to each person's comfort zone. We left around 3 pm and took the Cremallera back down to the train station and transferred to the main train. Back to the hotel by 5 pm.
If you need to have a guided tour of Monserrat, there is a tour company that picks you up in their van for a half day trip to Monserrat and a winery. We researched it, but felt it was too expensive and too time limiting for us.

As for a bicycle tour, I am an avid cyclist, but The only place I would want to ride a bike in Barcelona ( and the traffic) is along the waterfront on the bicycle/pedestrian path.
The public transportation is excellent. We took both the buses and the metro to all the major sites.

The guided tours I would recommend are specific to the sites. We did a guided tour of Parc Guell, the guided night tour of Casa Mila (La Pedreda) and a runner bean tour of the Bari Gotic.. Use Rick''s book to tell you what is important to see on the Las Ramblas. No guide needed there.

Good luck in your planning. We are taking the RS Best of Spain In October 2022. We have spent a week in Barcelona previously, so this time we are arriving a week early and going to see some of the less well known tourist sites on our own and renting a car to visit Girona, and the Dali Museum in Figures and staying several nights in Cadaques to visit the Dali house.

Thanks everyone!

Any downside to doing Monserrat on a Sunday?