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Organic nanocrystals of 1,3,5-triphenyl-2-pyrazoline (TPP) with a series of sizes were synthesized by reprecipitation method. The luminescence quantum efficiency of TPP nanocrystals increases from 24.2% for the nanocrystals with an average size of 300 nm to 34.6% for those with an average size of 20 nm. Surface capping by polyvinyl pyrrolidone (PVP) will improve the quantum efficiency of TPP nanocrystals. The size-dependence and capping-induced variation of the luminescence quantum efficiency was elucidated in viewpoint of aggregation quenching and the equilibrium between the TPP monomers and the aggregates in TPP nanocrystals.