Near-infrared spectroscopy (NIRS) can measure tissue blood content and oxygenation; however, its use for adult neuromonitoring is challenging due to significant contamination from their thick extracerebral layers (ECL; primarily scalp and skull). This report presents a fast method for accurate estimation of adult cerebral blood content and oxygenation from hyperspectral time resolved NIRS (trNIRS) data. A two-phase fitting method, based on a two-layer head model (ECL and brain), was developed. Phase 1 uses spectral constraints to accurately estimate the baseline blood content and oxygenation in both layers, which are then used by Phase 2 to correct for the ECL contamination of the late-arriving photons. The method was validated with in silico data from Monte-Carlo simulations of hyperspectral trNIRS in a realistic model of the adult head obtained from a high-resolution MRI. Phase 1 recovered cerebral blood oxygenation and total hemoglobin with an accuracy of 2.7 ± 2.5 and 2.8 ± 1.8%, respectively, with unknown ECL thickness, and 1.5 ± 1.4 and 1.7 ± 1.1% when the ECL thickness was known. Phase 2 recovered these parameters with an accuracy of 1.5 ± 1.5 and 3.1 ± 0.9%, respectively. Future work will include further validation in tissue-mimicking phantoms with various top layer thicknesses and in a pig model of the adult head before human applications.