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The performance of organic photovoltaics (OPVs) has rapidly increased. Yet, achieving long-term stability in the nano-morphology and thereby sustaining device performance remains challenging. Herein, we show that incorporating in-situ-forming cross-linked thermoset (CLT) matrices into the bulk heterojunction blends is a simple, general, and efficient strategy for high-performing and resilient OPVs. Our simulations and experimental data prove that these high-modulus CLT matrices featuring hydrogen-bonding interactions can freeze the nano-morphology, resulting in long-term thermal and photostable OPV devices. We demonstrate that this approach works efficiently with eight different blends and show that OPV devices can withstand 85°C for 1,000 h without losing performance. Blends with CLT matrices double the energy generated from OPV devices, showing an energy density output of 4,054 mW⋅h cm−2over an 11-week operating period under outdoor conditions. This methodology opens avenues for both developing new thermoset networks for OPV and their use in other optoelectronic applications.