Cost-effective and robust energy storage systems have attracted great attention for portable electronic devices. Three-dimensional electrodes can effectively enhance the charge transfer, increase the mechanical stability and thus improve the electrochemical performance upon continuous charge-discharge. The earth abundant halloysite nanotubes (HNTs) have shown immense potential in constructing nanoarchitectural composites. Here, we first demonstrate the development of hybrid composite of nickel sulfide (Ni3S2) and HNTs with glucose as binders for efficient energy storage in supercapacitor. The surface sulfhydrylation of HNTs and glucose-assisted hydrothermal reaction are crucial for the preparation of well-structured composite. Due to the synergistic effect between components, the Ni3S2/HNTs@HS composite electrode delivers a capacity of 450.4Cg−1 and high retention of 82.6% over 2000 cycles in three-electrode supercapacitors. Moreover, the Ni3S2/HNTs@HS//Whatman paper//Ni3S2/HNTs@HS two-electrode symmetric supercapacitor exhibits a maximum potential window of 1.3V, with a capacity of 250Cg−1 and performance loss of only 18.2% over 2000 cycling at 1Ag−1. A maximum energy density of 79.6 Wh kg−1 is achieved at a power density of 1.03kWkg−1. Such excellent energy storage performance suggests the great potential of Ni3S2/HNTs@HS for high-efficiency energy storage systems.