Multispectral imaging (MSI) is a valuable sensing modality for applications that require detecting a scene’s chemical characteristics. Existing MSI techniques utilize a filter wheel or color filter arrays, which are subject to reduced temporal or spatial resolution. In this work, we present a cephalopod-inspired multispectral organic sensor (CiMOS) based on geometric phase lenses (GPLs) and organic photovoltaics (OPVs) to enable aberration-based color sensing. We mimic the approach by which animals with single-type photoreceptors perceive colors via chromatic aberration. The intrinsic chromatic aberration of GPLs allows for multispectral sensing by stacking precisely patterned OPVs within specific spectrally dependent focal lengths. We provide simulations and a proof of concept of the CiMOS and highlight its advantages, including its simple design and snapshot multi-color detection using only a single axial position. Experimental results demonstrate the sensor’s ability to detect four colors with full width at half maximum spectral resolution as low as 35 nm.