yes, you will fry the step up circuit if not the led, then the circuit. For more brightness 10% maybe, try using NIMH AAA or Lithium primary AAA batteries.
Unless you are slapping a Luxeon in there I wouldnt mess with the little Garrity. It is what it is.
Just currious, is the Garrity light using an uncut nichia? If it has a nice reflector you might get a much nicer beam by hand cutting your 5mm LED so it fires to the sides making use of the reflector. That would be a worthy mod.
If you really wanna have some fun get a set of AAA LIthium Ions from AW with a charger and driect drive the sucker. It'd be about twice as bright. or replace the nichia with a SMJLED for maybe 50% increase in brightness.. both options are spendy though. Whatever you do dont direct drive the SMJLED with the 3.7volt LIthium.
just spreading the word.