Deficient intrinsic species and suppressed Curie temperatures (Tc) in two-dimensional (2D) magnets are major barriers for future spintronic applications. As an alternative, delaminating non-van der Waals (vdW) magnets can offset these shortcomings and involve robust bandgaps to explore 2D magneto-photoconductivity at ambient temperature. Herein, non-vdW α-MnSe2 is first delaminated as quasi-2D nanosheets for the study of emerging semiconductor, ferromagnetism and magneto-photoconductivity behaviors. Abundant nonstoichiometric surfaces induce the renormalization of the band structure and open a bandgap of 1.2 eV. The structural optimization strengthens ferromagnetic super-exchange interactions between the nearest-neighbor Mn2+, which enables us to achieve a high Tc of 320 K well above room temperature. The critical fitting of magnetization and transport measurements both verify that it is of quasi-2D nature. The above observations are evidenced by multiple microscopic and macroscopic characterization tools, in line with the prediction of first-principles calculations. Profiting from the negative magnetoresistance effect, the self-powered infrared magneto-photoconductivity performance including a responsivity of 330.4 mA W-1 and a millisecond-level response speed are further demonstrated. Such merits stem from the synergistic modulation of magnetic and light fields on photogenerated carriers. This provides a new strategy to manipulate both charge and spin in 2D non-vdW systems and displays their alluring prospects in magneto-photodetection.