I own both....Purchased a 09 Venza 3.5 AWD in Aug. I got my Crosstour 4WD + Navi two weeks ago.
I have put 25k miles on the Venza and my Wife wanted to take it over when she returned her leased 06 Nissan Altima. The Venza is a very good car, drives very nice +great acceleration with the 3.5 v6, nice mix of interior room and space without that big vehicle feel. I drove in snow all winter between Michigan/Ohio/Penn and the Venza was excellent in the snow. My last car was an Audi A4 Quattro and that was great in snow, but the Venza is as good if not better due to the latest electronic assist features. So why did I get the Crosstour? I was about to get an Audi A5 and decided to check out the Crosstour as I had second thoughts on the A5 due to the amount of mileage I will put on each year and it was going to cost me @45k. I started to look at alternatives including the Buick Lacrosse, Audi A3, Subaru Legacy, BMW 3-series XDrive and Acura TL SH-AWD. I wanted a car, and AWD was a requirement. In the end, The Crosstour is very similar to the Acura TL and was 5k less for just about the same features. Also insurance is very low I think due to the classification of a Wagon.
To sum it up, you would not make a bad decision with the Venza. It's just a different vehicle then the Crosstour. The Crosstour to me is more car like and the Venza is more to the SUV side of the spectrum. The Crosstour is posting better MPG compared to my 3.5 v6 Venza thanks to VCM.