We report on a recent spectral line survey of the planetary nebula (PN) NGC 7027 using the Arizona Radio Observatory (ARO) 12 m telescope and the Heinrich Hertz Submillimeter Telescope (SMT) at millimeter wavelengths. The spectra covering the frequency ranges 71-111, 157-161, and 218-267 GHz were obtained with a typical sensitivity of -->rms < 8 mK. A total of 67 spectral lines are detected, 21 of which are identified with 8 molecular species, 32 with recombination lines from hydrogen and helium, and 14 remain unidentified. As the widths of emission lines from CO, other neutral molecules, molecular ions, and recombination of H+ and He+ are found to be different from each other, the line strengths and profiles are used to investigate the physical conditions and chemical processes of the neutral envelope of NGC 7027. The column densities and fractional abundances relative to the H2 of the observed molecular species are calculated and compared with predictions from chemical models. We found evidence for overabundance of N2H+ and underabundance of CS and HNC in NGC 7027, suggesting that X-ray emission and shock waves may play an important role in the chemistry of the hot molecular envelope of the young PN.