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We have recently introduced a novel methodology for the noninvasive analysis of the structure and composition of human skin in vivo . The approach combines pulsed photothermal radiometry (PPTR), involving time-resolved measurements of mid-infrared emission after irradiation with a millisecond light pulse, and diffuse reflectance spectroscopy (DRS) in the visible part of the spectrum. Simultaneous fitting of both data sets with respective predictions from a numerical model of light transport in human skin enables the assessment of the contents of skin chromophores (melanin, oxy-, and deoxy-hemoglobin), as well as scattering properties and thicknesses of the epidermis and dermis. However, the involved iterative optimization of 14 skin model parameters using a numerical forward model ( i.e. , inverse Monte Carlo - IMC) is computationally very expensive. In order to overcome this drawback, we have constructed a very fast predictive model (PM) based on machine learning. The PM involves random forests, trained on ∼9,000 examples computed using our forward MC model. We show that the performance of such a PM is very satisfying, both in objective testing using cross-validation and in direct comparisons with the IMC procedure. We also present a hybrid approach (HA), which combines the speed of the PM with versatility of the IMC procedure. Compared with the latter, the HA improves both the accuracy and robustness of the inverse analysis, while significantly reducing the computation times., Competing Interests: The authors have no conflicts of interests to declare., (© 2020 Optical Society of America under the terms of the OSA Open Access Publishing Agreement.)