Achieving high areal capacity current lithium-ion batteries (LIBs) become a significant challenge in fields of consumer electronics, vehicle electrification, and aerospace. One of the most important strategies to achieve high areal capacity is developing unique electrodes through a hybridization blueprint. Herein, we demonstrate the design of 3D self-supportive pseudocapacitance core-shell architecture electrode as high areal capacity anode for LIBs. The pseudocapacitive 1D−VN/2D−MoS2 nanowires/nanosheets core/shell coated on free-standing 3D carbon fiber textile (CFT) (denoted CFT-VN@MoS2) exhibit high areal capacity of 6.80 mAh cm−2 at 0.5 mA cm−2, attractive rate performance of 1.27 mAh cm−2 at 17.0 mA cm−2 as well as 80% capacitive contribution at 1.5 mV s−1. The excellent storage performance of CFT-VN@MoS2 over CFT-VN and CFT-MoS2 anodes can be related to the synergistic effect of the dual pseudocapacitive storage mechanism of both VN and MoS2 and tailored 3D nanoarchitecture design. This present work urges an appropriate approach to improve the areal capacity and rate capability of self-supporting electrodes and may also be applicable to other hybrids for LIBs and beyond.