When the gearbox is completely stalled, the power will be close to zero, since no work is being done, all of the energy is being converted to heat. Maximum electrical power transfer will occur when the load resistance is equal to that of the motor. Maximum efficiency is a more tricky one, since efficiency goes down, when the current is very high due to increased I2R losses, yet it's also low under light loads, as the frictional losses in the gearbox, motor bearing, commutator and eddy losses in the armature dominate.
Use a boost converter to charge the capacitor to as higher voltage, as it's rated to.
When discharging, use a buck converter to provide a constant current to the LED, as the capacitor discharges.
The bridge rectifier should of course be made from Schottky diodes to minimise the forward voltage drop.