Low acid resistance of LTA zeolite membranes has restricted their wider application in dehydration of organics. Herein, an effective and facile route was proposed to enhance the acid stability of LTA zeolite membrane. Organosilica BTESE layer was deposited on the surface of the defective LTA zeolite membrane aiming at combining the high hydrophilicity of LTA zeolite membrane with good acid resistance and selectivity of BTESE. FT-IR, SEM, XRD and EDX showed that BTESE layer was coated on the surfaces of LTA membrane. The effects of coating circle and concentration of BTESE sol on the separation performance were investigated in detail. The obtained BTESE/LTA composite membrane maintained stable and high separation performance within 240 min for the separation of 90 wt% ethanol/water mixture at pH=3, indicating the BTESE/LTA membrane would be potential candidate for dehydration of organics in acidic condition.