In this paper, we present and analyze a compact inner-wall grating slot microring resonator (IG-SMRR) with the footprint of less than 13 μm × 13 μm on the silicon-on-insulator (SOI) platform for label-free sensing, which comprises a slot microring resonator (SMRR) and inner-wall grating (IG). Its detection range is significantly enhanced without the limitation of the free spectral region (FSR) owing to the combination of SMRR and IG. The IG-SMRR has an ultra-large quasi-FSR of 84.5 nm as the detection range, and enlarged factor is up to over 3 compared with the conventional SMRR. The concentration sensitivities of sodium chloride solutions and D-glucose solutions are 996.91 pm/% and 968.05 pm/%, respectively, and the corresponding refractive index (RI) sensitivities are 559.5 nm/RIU (refractive index unit) and 558.3 nm/RIU, respectively. The investigation on the combination of SMRR and IG is a valuable exploration of label-free sensing application for ultra-large detection range and ultra-high sensitivity in future.