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A new sol-gel process is applied to fabricate the BST (BaxSr1(xTiO3) sol and nano-powder of La-Mn-Al co-doping with Ba/Sr ratio 65/35, and the BST thick film is prepared in the Pt/Ti/SiO2/Si substrate. The powder and thick film are characterized by X-ray diffraction and transmission electron microscope. The influence of La-Mn-Al co-doping on the dielectric properties and micro-structure of BST thick film is analyzed. The results show that the La, Mn, and Al ions can take an obvious restraint on the growth of BaSrTiO3 grains. The polycrystalline particles come into being during the crystallization of thick film, which may improve the uniformity and compactness of thick film. The influence of unequal-valence and doping amount on the leakage current, dielectric loss, and dielectric property are mainly discussed. The dielectric constant and dielectric loss of thick film are 1200 and 0.03, respectively, in the case of 1mol% La doping, 2mol% Mn doping, and 1mol% Al doping.