I wouldn't waste to much time pondering over whether one is an SUV and the other a crossover, both are pretty meanigless terms for essentially the same type of car.
The problem i'd have with the VW would be regarding the 1.5TSI engine. Are the kangarooing issues fixed or not?. Also, you haven't mentioned transmission, but if you wanted auto, i'd rule out the VW there too unless you planned to change cars before the warranty was up.
The 'problems' with the Peugeot is not going to be problems for everyone. The first of these does polarise opinion somewhat, Peugeot's 'i-cockpit'. You have a very small steering wheel which you should set low in your lap so you view the instruments over the top of it. Some folk get along fine with it, others don't, so you really need to try it (assuming you haven't already) before comitting as you may hate it!. Second potential issue is having most of the controls, including heating and ventilation on the touchscreen. Again, some don't mind this, particularly the type who leave them at the same settings all the time, but quite distracting if you want or need to change the settings on the move.
The comparison to the Volvo is interesting, as the Peugeot, in exterior dimensions is mid way between the T-Roc and XC60. But, it actually has a bigger boot at 513 litres vs 483 litres (the T-Roc is 445 litres). I was surprised at how meagre the Volvo's boot is for that size of car. But that in turn leads me to suspect that both your suggestions, as second (smaller) cars are bigger than you actually need.
If it was my choice, i'd be looking at a size down in both cases, the VW T-Cross vs Peugeot 2008. In the case of the VW, i'd also be looking at its VAG group stablemates, the Seat Arona and Skoda Kamiq. And in all three cases, the 1.0TSI (115bhp) would be my engine choice (with manual gearbox). Actually the 2008 is closer in size to the T-Roc, so i'd maybe swap the 2008 for the Citroen C3 Aircross (1.2 110bhp).
But in this particular class of car there are a huge amount of contenders, including the Ford Puma (the one to go for if you like to throw the car around a bit!).
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