I used to play a lot of Fallout 4 with gyro aiming on the Steam Controller, there was a lot of downtime between fights and gunplay didn't require perfect precision, which was great for learning how the controller felt. I'd find that I'd sit back with my hands on my lap, tilting the controller very slightly up and down for vertical aim and unconsciously using my foot to rotate the chair for horizontal. Once I got used to how it worked (including setting the gyro to only activate while the left trigger was held and fine-tuning the sensitivity) it became natural. My body just kind of figured it all out in the most comfortable way.