Highly solar light-absorbing poly(vinyl alcohol) (PVA) nanocomposite films have garnered wide attention in fields such as flexible optoelectronics, solar energy harvesting, and photothermal therapy. However, fabricating PVA nanocomposite films with a broad spectrum of solar absorption using cost-effective and non-toxic nanofillers remains challenging. Herein, nanocomposite films of PVA incorporating various concentrations of mixed-phase 2D MoSe2 nanosheets (i.e., a combination of the 2H and 1T phase) were prepared using a solution casting technique. Scanning electron microscopy (SEM) shows homogenous dispersion of MoSe2 nanosheets in the PVA matrix even at higher concentrations, while atomic force microscopy (AFM) reveals increasing surface roughness with increasing MoSe2 content, reaching a plateau after 20 wt%. With the increase in the concentration of MoSe2, the nanocomposite films exhibit interesting light absorption characteristics reaching their highest absorption (average 94.9%) at 40 wt% MoSe2. The incorporated mixed-phase MoSe2 nanosheets induce a significant change in the energy levels of the PVA matrix, which is reflected in the reduced optical band gap energy (2.63 eV) at 40 wt% MoSe2 against pure PVA (5.28 eV). The excellent light absorption of PVA nanocomposite films across the entire range from 250 nm to 2500 nm is attributed to the thin 2D structure of MoSe2 and the presence of its mixed phase.