A new organic dye, trans-4-[p-(N-hydroxyethyl-N-ethylamino)styryl]-N-methyl-pyridinium p-toluene sulfonate (HEASPS) has been synthesized and its structure has been determined. Pumped with a 1064 nm, 50 ps laser pulses, 0.05 mol/L HEASPS/DMF solution showed the two-photon pumped (TPP) output/input efficiency of 9.1% which is higher than that of known TPP laser dyes trans-4-[p-(N-hydroxyethyl-N-methylamino) styryl]-N-methylpyridinium iodide (ASPI) and trans-4-[p-(N-hydroxyethyl-N-methylamino) styryl]-N-methylpyridinium p-toluene sulfonate (HMASPS) at the same experimental conditions.