Nearly 50% of global primary energy consumption is lost as low-temperature heat. λ-Ti3O5 holds promise for waste heat harvesting and reuse; however, achieving reversible phase transitions between its λ and β phases under accessible conditions remains a major challenge. Here, we proposed a simple laser method that incorporates element substitution for sub-minute synthesis (20–60 s) of λ-MxTi3-xO5 (M = Mg, Al, Sc, V, Cr, Mn, or Fe, 0.09 ≤ x ≤ 0.42). In particular, aluminum-substituted λ-AlxTi3-xO5 demonstrated the lowest energy barrier, with a transition pressure of 557 MPa and temperature of 363 K. Notably, compression of the (001) crystal plane could reduce the transition pressure to only 35–40 MPa, enabling the applicability of λ-AlxTi3-xO5 for wide applications in heat recovery and future lunar explorations. Reversible phase transitions between the β and λ phases of Ti3O5 under moderate conditions still remain challenging. Here, the authors report elemental substitution and (001) crystal plane compression strategies to achieve accessible heat storage