What precautions should travelers take in Spain/France?

Barcelona had more pickpocketing than any other city I've gone to for a conference. One year every single person I spoke to had a theft story. One person had been mugged, a woman had her laptop bag slit in the elevator and the laptop removed without her knowledge, and I was in a group of 4 who ate in a sandwich shop with our bags at our feet and stood up to go only to realize one of the bags was gone. That said, the trouble all happened at the convention centre - word was that pickpocket gangs came in to town when big conferences were on - or at night on Las Ramblas. I never felt in danger on Las Ramblas at night (and I have been known to feel in danger in Toronto at night, so my danger bar is set awfully low) but I was never completely alone: usually I had two or more men with me, and sometimes I was in a group of 20 or more. We took the subway without incident, btw.

My tip for those tourist-harassers is to learn to say no thankyou in the local language. It made all the difference for me in Paris and I'm sure that holds elsewhere. Don't sound flustered or scared; sound bored, like "geez here I am just going to work as usual and you idiots are treating me like a tourist." Say it like you've said it a thousand times. The one time I said "no thankyou" instead of "non merci" to the Eiffel Tower crowd I really was shocked at the aggressive "sell" they switched into. It had been a total non-issue up to then because I had spoken French when approached.

I have to say that Las Ramblas in Barcelona is the most thief-ridden part of the world I've been to. Moreso than all the other big cities I've been to in Europe east or west, Central America, or India. In the week I was there I either saw at least one person robbed or met at least one person who'd been robbed each and every day, some involving violence. It really is a great city though. You may be able to use it as a place to "toughen up".

(The main train stations in Amsterdam and Milan were next worse for me)

The Pyrénées will be perfectly relaxing and stress free though. Visit Andorra if you can while you're there.

I don't like traveller's safety wallets that go around your neck or like a belt. When you need to access them you have to find a totally hidden place or reveal to the world that you're carrying a precious goldmine. Dress cheap and drab. Leave the most fancy and valuable stuff you won't need in the hotel. I prefer cheap digital cameras over DSLR's for this very reason. Just have enough money in your wallet for what you'll need. Not in your back pocket. Don't walk with your fists jammed into your pockets either. Adopt a hardened "seen it all" look. Sometimes you can learn it from the locals. Scan crowds for dodgy types. Don't trust anybody that wants to be your friend in a dodgy area. Make eye contact with safe looking couples and families. Learn the words for "thief" and "help" in the local language. The locals have also been robbed and also hate thieves and they will be on your side.

I think I've made it sound too scary. Sorry for that. Those are my techniques for the medina of Casablanca at dusk so you won't have to go so far (-:

And have a great time!

Common sense invite to take precautions in big cities and touristic places. But this should not prevent you from visiting great sites. Just avoid to show your high-end smartphone to everyone in the subway or in crowds.

Anyways, The Pyrénées region is very rural and exempt of the kind of harrassments you experienced in Milano. Even Toulouse is safer. Enjoy your trip.