Northern Spain

While I haven’t been to either, I have Rupit and Passarel·la-mirador de Castellfollit de la Roca on my to visit list. If you like castles there’s Castell de Cardona.

In the French Basque area, Ascain, Ainhoa, Espellette, and Saré are a few of the charming villages.

Puigcerda (poo cher DAH) and La Seu d'Urgell are both attractive places. Puigcerda is a hill town in the Cerdanya valley that can be quite hot in the summer; I'm guessing October would be more comfortable.

I'm a fan of the French Yellow Train through the Pyrenees (Latour de Carol to Villefranche-de-Conflent). You can pick it up at Bourg Madame, just across the border from Puigcerda.

It's probably well off the route you're thinking of, but the small medieval town of Besalu west of Girona is worth a stop. It has a fortified bridge.

On the Catalan side of the Pyrenees there are plenty of quaint villages and other POIs one can visit, a small selection:

Rupit
Ribes de Freser
Queralbs
Camprodon
Vielha
Aigüestortes i Estany de Saint Maurici National Park
Vall de Boí
Vall de Núria

Thank you for the Yellow Train suggestion. It looks fantastic, but is too far from Barcelona for a 3-4 day trip. Do you have any suggestions that are closer to Barcelona.
We do want to visit Besalu and Girona, either by car or by train or on an escorted tour. What is your recommendation?

What are POIs?
I am going to research the villages that you mentioned.
Thank you.

Points, or places of interest.

Thank you for the clarification. It makes sense.

Any Barcelona hotel suggestions?

I opted to spend several nights in Girona back in 2017. I figured there was enough to see there that a day trip wouldn't cut it. There's bus service from Girona to Besalu. I understand you can also travel directly from Barcelona to Besalu by bus, but that doesn't seem a good way to go if you want to see both Besalu and Girona. Girona is also an excellent base for a day trip to Figureres (Dali Theatre-Museum) and/or Cadaques.

I haven't tried to figure out the precise timing, but one can take the train from Barcelona up to Perpignan in France, then change to a westbound train that links up with the Yellow Train, ending up in Bourg Madame very near Puigcerda. I've done all parts of that trip, but on two different occasions, so I just don't know whether one could make it all the way to Puigcerda by way of France in one day. And of course one would not have a car.

It is wonderful to hear from people like you. Thank you for all of your good advice. As much as we would like to take the yellow train, it seems a bit too much for this trip. However we will take your advice on everything else. Thanks again.

Yes, just points of interest, my recommendations range from hamlets in the deep mountains, to villages in the foothills, and larger towns. To clarify Girona is a full on city while Besalú is a town of a few thousand. If you want to see the real Pyrenees villages lost in time (I'm thinking less than 500 pop) you'll probably need to rent a car.

One notable exception is from Barcelona one can take the regional R3 train up to the Pyrenees mountain town of Ribes de Freser and then switch to the rack railway up to smaller medieval stone village of Queralbs and then on to the Vall de Núria sanctuary for some amazing hiking. This is the train line https://en.wikipedia.org/wiki/R3_(Rodalies_de_Catalunya)
then switch to this one at Ribes de Freser
https://en.wikipedia.org/wiki/Vall_de_N%C3%BAria_Rack_Railway

Thank you once again. I look forward to investigating your recommendations tomorrow.

Boi , Tull, Broto, Ainsa, Torla, Benasque, Bielsa All in Spanish Pyrenees. More than enough for 3-4 days. Gotta have a car.
Buen viaje Brad

Thank you for the recommendations. I will enjoy looking up the towns today.

I know your post was some time ago but perhaps you haven't worked everything out yet. We were in Barcelona for the second time four years ago and did a bus tour to Girona and Figueres from there. It's not something we usually do, preferring to drive ourselves and do things independently. We wandered Girona by ourselves and it was delightful but we had a guide for Figueres which was excellent. She opened our eyes and hearts so much. I know I would not have appreciated the wonder of the place nearly as much without her. From memory it cost about E75 for the whole day and was well worth it (probably more now...) I do like the idea of staying in Girona for a few days, we just haven't had the time. There is soooo much to do and see in Spain.