Abstract We describe continuous-wave (cw) intracavity frequency-doubling experiments performed with a Cr:LiCAF laser. The Cr:LiCAF crystal is home-grown and had passive losses below 0.15% per cm. The laser is pumped by two recently-developed high-brightness tapered diodes, providing a total pump power of 2 W at 680 nm. The Cr:LiCAF laser generated up to 585 mW of cw output power around 800 nm with 43% slope efficiency at an absorbed pump power of 1.4 W. The low passive losses of the crystal enabled storage of up to 380 W of intracavity laser power using a 0.07% transmitting output coupler, demonstrating suitability of Cr:LiCAF gain media for intracavity nonlinear conversion experiments. By performing intracavity frequency doubling with a BBO crystal, cw second-harmonic powers as high as 265 mW around 400 nm have been realized with optical-to-optical conversion efficiencies as high as 13.3%. To our knowledge, these are the highest cw frequency-doubled laser powers and conversion efficiencies obtained from Cr:Colquiriites to date. Moreover, obtained efficiencies are superior compared to what have been achieved with similar Ti:Sapphire systems, due to lower passive losses of Cr:LiCAF crystal. These results demonstrate the appropriateness of Cr:LiCAF gain media as a high-power tunable cw radiation generator in 375–435 nm region.