The SST-90 spec sheet here shows 3.25 V @ 3.15 A typical, but if I want a moonlight mode can I just run the same forward voltage (3.25 V) at a lower amperage (say, 500 mA)? Or is there another consideration I haven't considered?
Voltage is linked to amperage, so it's physically impossible for you to run it at two currents but keep the same voltage. As you decrease the current, the Vf will also decrease as per the graph on page 10.