Single crystals of polar LiCrP2O7 were grown by using a top-seeded solution growth method. In addition to the crystal structure, detailed magnetic measurements reveal anisotropic magnetic behavior with a spin-flop transition. Piezoelectric, polarization, and heat capacity measurements were also taken on the single crystals. Powder second-harmonic generating measurements, using 1064 nm radiation, revealed type 1 phase-matching behavior with an efficiency of approximately 30 X alpha-SiO2.