I feel long rides exclusively in my quads, should my calf muscles be doing more work?
I don't think you have a problem here. Physiologically, your thighs are the engine room of your legs. They are designed for endurance and power and can keep working at a high output for extended periods of time.

Your calves are more for short bursts of power, such as jumping or sprinting. They can't sustain high power output for any length of time. In distance cycling, your calves should be fairly passive. Attempting to work them harder will probably just result in fatigue and injuries.