Ni(OH)2 is recognized to be a promising material to detect hydrogen peroxide (H2O2), however, the fabrication method and electrocatalytic performances of suitable Ni(OH)2 structures are still in progress. In this work, we present a facile approach to in situ fabricate highly accessible Ni(OH)2/K-Ti-O composites by hydrothermally treating NiTi foil in 5M KOH solution. Based on systemic characterizations, the Ni(OH)2 appears nanoflakes, meanwhile the K-Ti-O shows nanowires in shape, which are randomly mixed together. Serving as a binder-free non-enzymatic sensor, the Ni(OH)2/K-Ti-O/NiTi foil electrode exhibits remarkable electrocatalytic activity towards hydrogen peroxide (H2O2) with a high sensitivity of 4278μAmM−1 cm−2 from 5μM to 1mM, and 1522μAmM−1 cm−2 from 1mM to 5mM. Further, the electrode can be demonstrated to have excellent selectivity, fast response, and long-term stability towards the H2O2 detection. It is found that the Ni(OH)2 plays a critical role with the synergistic effects of K-Ti-O. All our impressive performances indicate that the Ni(OH)2/K-Ti-O composites are promising electrode materials for non-enzymatic H2O2 sensors.