This paper presents a novel principle for intraocular pressure (IOP)-sensing (monitoring) based on a pressure-sensitive soft composite in which a dual optical signal is produced in response to impulsive pressure input. For the initial assessment of the new IOP sensing principle, a human eye is modeled as the spherically shaped shell structure filled with the pressurized fluid, including cornea, sclera, lens and zonular fiber, and a fluid-structure interaction (FSI) analysis was performed to determine the correlation between the internal pressure and deformation (i.e., strain) rate of the spherical shell structure filled with fluid by formulating the finite element model. The FSI analysis results for human eye model are experimentally validated using a proof-of-conceptual experimental model consisting of a pressurized spherical shell structure filled with fluid and a simple air-puff actuation system. In this study, a mechanoluminescent ZnS:Cu- polydimethylsiloxane (PDMS)-based soft composite is fabricated and used to generate the dual optical signal because mechanically driven ZnS:Cu/PDMS soft composite can emit strong luminescence, suitable for soft sensor applications. Similar to the corneal behavior of the human eye, inward and outward deformations occur on the soft composite attached to the spherical shell structure in response to air puffing, resulting in a dual optical signal in the mechnoluminescence (ML) soft composite.