Ageing characteristics of the metastable bcc γ-phase in U-9 wt.% Mo alloy, a candidate for high uranium density nuclear fuel for research and test reactors, have been investigated in this study. Analyses of the aged microstructures, employing X-ray diffraction and various microscopy techniques, revealed the decomposition mechanism of the metastable γ-phase to the stable α-U and γ′ (U 2 Mo) phases. A discontinuous precipitation reaction, leading to the generation of partially transformed cellular colonies with lamellae comprising of either the α-phase or the γ′-phase in γ-phase matrix, was found to be operative. The in situ transformation of γ interlamellar regions to the γ′-phase was noticed occasionally within the γ + α lamellar colonies. Thermodynamic analysis of the U-Mo system, using free energy-composition diagrams, could associate the observed attributes of the decomposition of γ-phase to the extent of Mo segregation and the chemical driving force required for the nucleation of α- and γ′-phases in the γ-matrix.