The size and operating energy of a nonlinear optical device are fundamentally constrained by the weakness of the nonlinear optical response of common materials. Here, we report that a 50-nm-thick optical metasurface made of optical dipole antennas coupled to an epsilon-near-zero material exhibits a broadband (∼ 400 nm bandwidth) and ultrafast (recovery time less than 1 ps) intensitydependent refractive index n 2 as large as −3.73 ± 0.56 cm 2 /GW. Furthermore, the metasurface exhibits a maximum optically induced refractive index change of ±2.5 over a spectral range of ∼ 200 nm. The inclusion of low-Q nanoantennas on an epsilon-near-zero thin film not only allows one to design a metasurface with an unprecedentedly large nonlinear optical response but also offers the flexibility to tailor the sign of the response. Our technique allows one to overcome a longstanding challenge in nonlinear optics, namely that of finding a material for which the nonlinear contribution to the refractive index is of the order of unity. It consequently offers the possibility of designing low-power nonlinear nano-optical devices with orders-of-magnitude smaller footprints.All-optical signal processing and computation are often hailed as breakthrough technologies for the next generation of computation and communication devices. Two important parameters of such devices, energy consumption and size, critically depend on 1 the strength of the nonlinear optical response of the materials from which they are made. However, materials typically exhibit an extremely weak nonlinear optical response. This property makes designing subwavelength all-optical active devices extremely difficult. Thus, all-optical active devices tend to have large footprints, which limits the integration density to many orders of magnitude smaller than what can be achieved in a state-of-the-art electronic integrated circuits [1,2]. Thus, materials with much stronger nonlinear optical responses are needed in order to enable integrated high-density on-chip nonlinear optical devices.Over the years several approaches have been explored to enhance the intrinsic nonlinear optical response of materials, including local field enhancement using composite structures [3,4,5], plasmonic structures [6,7], and metamaterials [8,9,10,11]. However, these techniques offer only limited control over the magnitude (and sign when applicable) of the wavelength-dependent nonlinear response, and typically involve a trade-off between the strength of the nonlinearity and the spectral position of the peak nonlinear response. It has been reported recently that materials with vanishingly small permittivitycommonly known as epsilon-near-zero or ENZ material -exhibit intriguing linear [12,13,14,15,16] and large nonlinear responses [17,18,19,20,21]. However, an ENZ material has a large nonlinear response over only a relatively narrow spectral range. Furthermore, the zero-permittivity wavelength, strength of the nonlinear response, and the losses depend on the optical properties of the ENZ material. In com...