In this paper, we developed a spectral emulator based on the Mapping Nearby Galaxies at Apache Point Observatory Stellar Library (MaStar) and a grouping optimization strategy to estimate effective temperature (T eff), surface gravity (log g), metallicity ([Fe/H]), and the abundance of alpha elements with respect to iron ([α/Fe]) for O-M-type stars within the Large Sky Area Multi-Object Fiber Spectroscopic Telescope (LAMOST) low-resolution spectra. The primary aim is to use a rapid spectral-fitting method, specifically the spectral emulator with the grouping optimization strategy, to create a comprehensive catalog for stars of all types within LAMOST, addressing the shortcomings in parameter estimations for both cold and hot stars present in the official LAMOST AFGKM-type catalog. This effort is part of our series of studies dedicated to establishing an empirical spectral library for LAMOST. Experimental results demonstrate that our method is effectively applicable to parameter prediction for LAMOST, with the single-machine processing time within 70 hr. We observed that the internal error dispersions for T eff, log g, [Fe/H], and [α/Fe] across different spectral types lie within the ranges of 15–594 K, 0.03–0.27 dex, 0.02–0.10 dex, and 0.01–0.04 dex, respectively, indicating a good consistency. A comparative analysis with external data highlighted deficiencies in the official LAMOST catalog and issues with MaStar parameters, as well as potential limitations of our method in processing spectra with strong emission lines and bad pixels. The derived atmospheric parameters as a part of this work are available via doi:10.12149/101402.