3/in-situ SiN passivation and Al2O3 gate dielectric were investigated. 20 nm thick high-k Al2O3 was deposited using a non-vacuum ultrasonic spray pyrolysis deposition method. Comparative studies between an in-situ SiN-passivated Schottky-gate HFET (sample A) and a composite Al2O3/SiN-passivated MOS-HFET were made. Electrical and deep-UV sensing characteristics for devices with different gate-drain separations (LGD) of 6 and 14 μm were also studied. Improved device performance has been obtained for the present sample B (A) with LGD = 6/14 μm separately, including maximum drain-source current density (IDS, max) of 634.4/463.1 (421.8/301.1) mA/mm, maximum extrinsic transconductance (gm, max) of 25.2/17.9 (19.1/15.2) mS/mm, on/off-current ratio (Ion/Ioff) of 7.4 × 107/5.4 × 107 (4.5 × 105/5.4 × 104), two-terminal off-state gate-drain breakdown voltage (BVGD) of -420/-480 (-320/-390) V, and three-terminal on-state drain-source breakdown voltage of 310/380 (220/300) V at 300 K. Superior spectral responsivity of 885.6 A/W under 250-nm deep-UV radiation has also been achieved for the present MOS-HFET.