When resetting the heading indicator to match the magnetic compass, do I need to use the compass deviation card?
Yes the DG is supposed to be set to the corrected magnetic indication whenever you set it, so you should mentally add or subtract the degree or two or three based on the closest segment on the card as a standard practice.

I agree with Michael however that it's not really that big a deal for VFR flying in the real world, especially in the age of GPS where you can just adjust heading based on GPS ground track on your phone or a tablet to go from A to B and you don't even really need to look at your compass (although, you might suddenly find you need it, so don't neglect it). 

If you were doing old fashioned dead reckoning navigation, precision in holding a heading is important.  Or in the IFR world where you have to fly headings in a clearance.  Even there though, the allowable calibration error on a compensated (that is, WITH the deviation accounted for) compass is +/- 10 deg (!), so the little 2 or 3 degree calibration card can be quite a bit off anyway and still be legal.