We report uniform liquid crystal (LC) alignment on a polyacrylamide (PAM) film via ion beam (IB) treatment. The IB incidence angle is adjusted from 15° to 75°. Physicochemical modifications caused by the IB process are investigated by atomic force microscopy and x-ray photoelectron spectroscopy. Low IB incidence results in biased and bumpy surfaces, whereas high IB incidence forms isotropic and smooth surfaces; both of these are unsuitable for uniform LC alignment. The 45° IB incidence induces anisotropic surface chemical reformations, and these modifications induce van der Waals forces between the LCs and modified PAM, thereby leading to uniform LC alignment. The LC alignment state is verified by polarized optical microscopy and pretilt angle. The electro-optical characteristic of the modified PAM showed excellent switching performance in twisted-nematic LC system. Thus, the IB-treated PAM film is a good candidate for LC alignment layers and suitable for LC device applications.