The characteristic properties of critically and noncritically phase-matched second-harmonic generation in crystalline lithium triborate (LiB3O5, LBO) grown in our laboratory are investigated. Angle-tuned critically phase-matched second-harmonic generation of near-infrared radiation is reported. Temperature-tuned noncritically phase-matched second-harmonic generation from 1.025 to 1.253-mu-n was achieved in the temperature range 190-degrees to -3-degrees-C. Spectrum-tuned noncritical phase matching at room temperature is also achieved at 1.215-mu-m. Large angular, temperature, and spectral acceptance bandwidths are obtained. The details of the LBO crystal growth process are also discussed.