In the current research, the delamination behavior under Mode I and Mode II loading for the hybrid carbon-thermoplastic fabrics in conjunction with novel liquid thermoplastic acrylic Elium® resin processable at ambient conditions was studied. The experimentation by incorporating doublers methodology, studying the performance under Mode I and Mode II loading, and understanding failure mechanisms using surface morphological fractography is deliberated. Hybrid Carbon-Ultra-high molecular weight polyethylene (UHMWPP)/Elium® composite has shown a 22.81% higher GIC and a 22.2% higher GIIC than Carbon-UHMWPP/Epoxy composite. On the contrary, the Carbon_Ultra-high molecular weight polypropylene (UHMWPE)/Elium® has shown an 11.11% higher Mode I critical energy release rate (GIC) and a 7.58% higher Mode II critical energy release rate (GIIC) than Carbon_UHMWPE/Epoxy composite. Hybrid fiber reinforced thermoplastic composites have shown severe plastic deformation of the matrix, rough fracture surface, and micro-cracks on the de-bonding surface, extensive fiber bridging, and crack branching which contributed to the improvement in the delamination behavior. Hybrid fiber architecture is also found to be detrimental by inducing crack arresting mechanisms including the tortuous crack path and the resin-rich pockets path due to the mismatch of the size of the fiber yarns.