Engineered micro-nano heterogeneous architectures for transition metal phosphide (TMPs) anode materials in lithium-ion batteries (LIBs) provide multifunctional active components. These components synergistically interact to address pivotal challenges of pronounced volume expansion and sluggish reaction kinetics within the electrode. Consequently, this engineering design approach significantly enhances the overall battery performance. In this study, a self-assembled approach is employed to integrate hybridized NiFe-PBA nanocubes with two-dimensional (2D) monolayer MXene (Ti3C2Tx), producing a heterostructured NiFeP/C@Ti3C2Tx composite. In this meticulously engineered architecture, the interface between the outer MXene layer and NiFeP embedded within the carbon matrix exhibits several distinct superiorities, such as rapid interfacial ion migration, multidirectional migration pathways, and strong spatial adaptability. The resulting non-uniform phase structure effectively mitigates electrode expansion and enhances electronic conductivity. Consequently, the NiFeP/C@Ti3C2Tx-15 composite demonstrates distinct performance advantages over NiFeP/C without MXene. The composite achieves a specific capacity of 689.4 mAh g⁻¹ at 200 mA g⁻¹ over 300 cycles, double that of NiFeP/C. Furthermore, density functional theory (DFT) calculations validate the electronic conductivity facilitated by the heterointerface between MXene and NiFeP, substantiating the strategic significance of the heterostructure in advancing high-performance anode materials for lithium-ion batteries.