To enable high-density optical storage, better storage media structures, diversified recording methods, and improved accuracy of readout schemes should be considered. In this study, we propose a novel three-dimensional (3D) sloppy nanostructure as the optical storage device, and this nanostructure can be fabricated using the 3D laser direct writing technology. It is a 900 nm high, 1 × 2 µm wide Si slope on a 200 nm SiO2 layer with 200 nm Si3N4 deposited on top to enhance reflectivity. In this study, we propose a reflected spectrum-based method as the readout recording strategy to stabilize information readout more stable. The corresponding reflected spectrum varied when the side wall angle of the slope and the azimuth angle of the nanostructure were tuned. In addition, an artificial neural network was applied to readout the stored information from the reflected spectrum. To simulate the realistic fabrication error and measurement error, a 20% noise level was added to the study. Our findings showed that the readout accuracy was 99.86% for all 120 data sequences when the slope and azimuth angle were varied. We investigated the possibility of a higher storage density to fully demonstrate the storage superiority of this designed structure. Our findings also showed that the readout accuracy can reach its highest level at 97.25% when the storage step of the encoded structure becomes 7.5 times smaller. The study provides the possibility to further explore different nanostructures to achieve high-density optical storage.