In this paper, results of positron annihilation lifetime spectroscopy (PALS) studies of MnFe2O4/MCM-41 nanocomposites in N2 and O2 atmosphere have been presented. In particular, the influence of manganese ferrite loading and gas filling on pick-off ortho-positronium (o-Ps) annihilation processes in the investigated samples was a point of interest. Disappearance of the longest-lived o-Ps component with τ5 present in the PAL spectrum of initial MCM-41 mesoporous material in the PAL spectra of MnFe2O4-impregnated MCM-41 measured in vacuum is a result of either a strong chemical o-Ps quenching or the Ps inhibition effects. The intensity I 4 of the medium-lived component initially increases, reaching a maximum value for the sample with minimum manganese ferrite content, and then decreases monotonically. Analogous dependence for the intensity I 3 of the shortest-lived component shows a maximum at higher MnFe2O4 content. Filling of open pores present in the studied nanocomposites by N2 or O2 at ambient pressure causes partial reappearance of the τ4 and τ5 components, except a sample with maximum ferrite content. The lifetimes of these components measured in O2 are shortened in comparison to that observed in N2 because of paramagnetic quenching. Anti-inhibition and anti-quenching effects of atmospheric gases observed in the MnFe2O4/MCM-41 samples are a result of neutralization of some surface active centers acting as inhibitors and weakening of pick-off annihilation mechanism, respectively.