Hybrid metal−organic cluster resist materials, also termed as organo-inorganics, demonstrate their potential for use in next-generation lithography owing to their ability for patterning down to ∼10 nm or below. High-resolution resist patterning is integrally associated with the compatibility of the resist and irradiation of the exposure source. Helium ion beam lithography (HIBL) is an emerging approach for the realization of sub-10 nm patterns at considerably lower line edge/width roughness (LER/ LWR) and higher sensitivity as compared to electron beam lithography (EBL). Here, for the first time, a negative tone resist incorporating nickel (Ni)-based metal−organic clusters (Ni-MOCs) was synthesized and patterned using HIBL and EBL at 30 keV. This resist comprises a nickel-based metal building unit covalently linked with the organic ligand: m-toluic acid (C 8 H 8 O 2 ). Dynamic light scattering confirmed a narrow size distribution of ∼2 nm for metal−organic cluster (MOC) formulations. High-resolution ∼9 nm HIBL line patterns were well developed at a sensitivity of 22 μC/cm 2 and at a significantly low LER and LWR of 1.81 ± 0.06 and 2.90 ± 0.06 nm, respectively. Analogous highresolution patterns were also observed in EBL with a sensitivity of 473 μC/cm 2 . Hence, the Ni-MOC-based resist investigated using HIBL and EBL elucidates the ability of its potential for the sub-10 nm technology node, under standard processing conditions.