Shopping in Spain

No offense, but that is kind of like asking what items you should shop for when visiting the US. What to shop for depends on your interests, budget, who you are shopping for, etc.

Since I like small and light, we went to a grocery store spice rack and bought a collection of spices we couldn't normally get at home (both for ourselves and our friends/family). We brought home a couple of other things but nothing really exciting.

Portuguese ceramics are beautiful and high quality. Coimbra is a big center for their manufacture, but they're widely available in other towns. There are also breath-takingly beautiful embroidered linens from Madeira (I think), but they are breath-takingly expensive. Characteristic ceramics are produced in various regions of Spain, as well; and leather goods can be a good buy.

While likely not exclusive to Spain, when we were in Andalucia we saw items made out of olive tree wood (bowls, cutting boards, etc.) that were beautiful. It was explained to us that olive trees are rarely cut down for the sole purpose of making wood items because fruit-bearing trees are far too valuable, which makes the wood a bit harder to come by. Large pieces will come with a large price tag because finding a big enough chunk of the wood to make big things is limited, but we saw several small to medium sized items (like the bowls) that were reasonable in price and gorgeous.

In May there was a nice artisan market along the river in Coimbra with various booths of local goods. Small ceramics pack well. Also in Nazare we bought a very nice table cloth. Also don't forget the Port! Not sure about spain heading there in a few weeks...

From Spain... a beautiful but useful fan.
From Portugal...definitely some sort of pottery or ceramic item.

Saffron and smoked paprika (pimentón).