The well known metrological linear squeezing parameters (such as quadrature or spin squeezing) efficiently quantify the sensitivity of Gaussian states. Yet, these parameters are insufficient to characterize the much wider class of highly sensitive non-Gaussian states. Here, we introduce a class of metrological nonlinear squeezing parameters obtained by analytical optimization of measurement observables among a given set of accessible (possibly nonlinear) operators. This allows for the metrological characterization of non-Gaussian quantum states of discrete and continuous variables. Our results lead to optimized and experimentally-feasible recipes for high-precision moment-based estimation of a phase parameter and can be used to systematically construct multipartite entanglement and non-classicality witnesses for complex quantum states.Introduction.-A central quest in quantum metrology is to relate the reduced variance of an observable to the possible enhancement of sensitivity in parameter estimation [1][2][3][4]. For instance, quadrature squeezing can enhance the sensitivity of homodyne interferometers beyond the shot-noise limit [1], as experimentally demonstrated with squeezed vacuum states of light [5,6] and atoms [7], and envisaged for thirdgeneration gravitational wave detectors [8,9]. Moreover, multi-mode squeezing can reveal mode entanglement [10][11][12][13][14][15] and Einstein-Podolski-Rosen correlations [16][17][18][19]. Squeezing of a collective spin [2] currently represents the leading strategy to obtain quantum-enhanced sensitivities in Ramsey interferometers [3], with direct applications to atomic clocks [20], magnetometers [21], and matter-wave interferometers [22]. Spin squeezing is also a witness of metrologicallyuseful multiparticle-entanglement [23][24][25][26] and Bell correlations [27][28][29]. Squeezing of linear observables of discrete [23][24][25][26][30][31][32][33][34][35][36][37] or continuous variables [38][39][40][41][42], e.g., collective spins or quadratures, has proven to be a successful concept to characterize the class of Gaussian quantum states with phase-estimation sensitivities beyond the classical limit [3], and is hereinafter indicated as metrological linear squeezing.Yet, some highly sensitive continuous-variable states are non-Gaussian [43][44][45][46] and Gaussian spin states form a small and non-optimal class of useful states for quantum metrology [47][48][49]. Non-Gaussian states further hold the promise of opening up classically intractable pathways for quantum information processing [50][51][52]. These perspectives have led to a growing interest in the generation of non-Gaussian quantum states in both discrete-and continous-variable systems [53] using nonlinear processes [54,55], photon-addition orsubtraction [56][57][58] or measurement techniques [44,45,59]. More refined tools are required to characterize highly sensitive non-Gaussian states, as the linear squeezing coefficient becomes too coarse to capture non-Gaussian features [54]. It would be highly desirable t...