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Abstract The current study confirms that modified carbon fiber reinforced polymer (CFRP) composites have higher fracture toughness than unmodified CFRP composites achieved by exploiting the synergistic effect of a polycarbonate (PC)/acrylonitrile butadiene styrene (ABS) blend in toughening the diglycidyl ether of bisphenol A (DGEBA) epoxy resin. The CFRP composite specimens are tested at near cryogenic temperatures using TMA, DMA, and microcrack analysis to determine the best‐suited concentration of ABS in the PC/ABS blend. TMA and DMA results, as well as microcrack analysis at cryogenic temperatures (CT), confirm that the blend 90/10 is effective in reducing the brittle nature of DGEBA resin and increasing bond strength, resulting in the fracture toughness enhancement of CFRP specimens at CT. Further investigation of 90/10 modified CFRP (90/10 m‐CFRP) and unmodified CFRP specimens using Mode II fracture using ENF test and SEM analysis reveal significant reduction in brittle characteristics of matrix with increase in elongation at failure and fracture surface morphologies confirm nano web‐like structures bridging the CF layers, proving to improve fiber/matrix bond strength. This study concludes the effectiveness of hybrid PC/ABS blend in synergistically‐modifying DGEBA resin for improved fracture toughness of CFRP laminates across a wide temperature range (−150°C to 150°C).