This paper presents full-scale experimental investigations on cross-laminated timber concrete composite (TCC) systems. The primary objective was to determine the stiffness, ultimate load-carrying capacity, and failure modes of TCC systems using three different shear connectors: self-tapping screws, steel kerf plates, and proprietary glued-in perforated steel plates. The secondary objective was to determine the effectiveness of shear reinforcement in the CLT panels. The TCC system was comprised of 245 mm thick, 7-ply CLT panels with a 150 mm concrete topping. A total of 24 half-span (4.6 m long) and 9 full-span (9.2 m long) CLT and TCC floor segments were tested under symmetric four-point bending as well as torsional bending. For all test series, the CLT panels were either unreinforced, or reinforced using self-tapping screws. The shear reinforcement increased rolling shear capacity which helped to avoid CLT shear failure. Adding the concrete topping increased the shear capacity by up to 167%. The tests showed that the floors with steel kerf plates exhibited the highest capacity and stiffness, while also being the most easy-to-install solution. The results from this research guided project-specific design decisions for “Limberlost Place”, a mass timber building for George Brown College, in Toronto, Canada.