Ultralow-power logic devices are next-generation electronics in which their maximum efficacies are realized at minimum input power expenses. The integration of ferroelectric negative capacitors in the regular gate stacks of two-dimensional field-effect transistors addresses two intriguing challenges in today's electronics; short channel effects and high operating voltages. The complementary-metal-oxide-semiconductor-compatible Hf0.5Zr0.5O2 (HZO) is an excellent ferroelectric material crystallized in a noncentrosymmetric o-phase. The present work is the first to utilize pulsed laser deposition (PLD)-grown phase-pure ferroelectric HZO to achieve steep slope negative capacitance (NC) in field effect transistors (FETs). A dual-step growth strategy is designed to achieve phase-pure orthorhombic HZO on silicon and other conducting substrates. The room-temperature PLD-grown amorphous HZO is allowed to crystallize using rapid thermal annealing at 600 °C. The polycrystalline orthorhombic HZO is further integrated with atomic layer deposition-grown HfO2 to achieve a stable NC transition. The stack is further integrated into the molybdenum disulfide channel to achieve steep switching and a hysteresis-free operation of the resulting FETs. The subthreshold swings of the FETs are 20.42 and 26.16 mV/dec in forward and reverse bias conditions, respectively.