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The 1064 nm optimal spatial phase matching (PM) direction for LaCa4O(BO3)3 (LaCOB) crystals was found to be (113.5°, 43.8°) with deff of 1.34 pm V−1, angular acceptance of 0.9 mrad cm and walk-off angle of 14.9 mrad, and more than a 56% second-harmonic generation (SHG) conversion efficiency was realized on a sample (4  ×  4 × 6 mm3) cut in this direction, by using a 1064 nm Nd : YAG pico-second laser. The angular noncritical phase-matching (A-NCPM) wavelengths along the y and z axes for LaxGd1−xCOB (x = 0.09, 0.13) crystals were measured. Using a nanosecond laser, the type-I single-pass A-NCPM SHG conversion efficiency along y axis reached 30.2% by taking advantage of the longer crystal sample (4  ×  4 × 27 mm3). [ABSTRACT FROM AUTHOR]