Nonlinear second harmonic optical activity of graphene covering a gold photon sieve was determined for different polarizations. The photon sieve consists of a subwavelength gold nanohole array placed on glass. It combines the benefits of efficient light trapping and surface plasmon propagation in order to unravel different elements of graphene second-order susceptibility χ (2) . Those elements efficiently contribute to second harmonic generation. In fact, the graphene-coated photon sieve produces a second harmonic intensity at least two orders of magnitude higher compared with a bare, flat gold layer and an order of magnitude coming from the plasmonic effect of the photon sieve; the remaining enhancement arises from the graphene layer itself. The measured second harmonic generation yield, supplemented by semianalytical computations, provides an original method to constrain the graphene χ (2) elements. The values obtained are | + | ≤ 8.1 × 10 pm²/V and | | ≤ 1.4 × 10 pm²/V for a second harmonic signal at 780 nm. This original method can be applied to any kind of 2D materials covering such a plasmonic structure.Besides its atomic thickness, graphene has become a new, challenging, playground for many kinds of photonic applications 1-3 , due to its outstanding electrical, mechanical and optical properties. For example, its ability to respond to an externally applied electric field makes graphene of special interest for electro-optic purposes. Its unique light absorption and high electric field confinement properties offer new potential -for instance in nonlinear spectroscopies, through efficient frequency conversion, with multiwave mixing mechanisms [4][5][6] .However, quantification of graphene nonlinear susceptibilities over metallic surfaces is still sparsely reported [7][8][9][10][11] . Quantitative data are of prime necessity to model processes such as frequency conversion in new types of hybrid devices 7 efficiently. In order to mend this gap, this letter proposes an original method combining experimental and numerical results to reconstruct the second-order susceptibility tensor of hybrid systems that are composed of 2D materials covering plasmonic structures. Here, the hybrid system is a photon sieve, i.e. a flat gold film, perforated according to a honeycomb nanohole pattern and coated with a graphene layer [12][13][14][15][16] . As shown hereafter, using a graphene-coated gold photon sieve enhances second harmonic (SH) conversion efficiency by up to two orders of magnitude, compared with bare flat gold, or, similarly, by up to an order of magnitude, compared with a bare gold photon sieve. This enhancement results from the propagation of surface plasmon polaritons (SPP) at the gold/graphene interface.Indeed, planar graphene in conjunction with metallic nanostructures enables localized electromagnetic hotspots to be created on the graphene sheet, thereby increasing light absorption by flat graphene above the classical value of 2.3% [16][17][18][19][20][21][22][23][24] . Moreover, it circumvents...