Vertically aligned MoS nanosheets (NSs) with exposed edges were successfully synthesized over a large area (∼2 cm). The NSs were grown using an ambient pressure chemical vapor deposition technique via rapid sulfurization of sputter deposited thick molybdenum films. Extensive characterization of the grown MoS NSs has been carried out using high resolution scanning and transmission electron microscopy (SEM & TEM). A special care was given to the TEM lamella preparation process by means of a focused ion beam to preserve the NS growth direction. The cross-section TEM measurements revealed the growth of densely packed, vertically aligned and straight MoS NSs. Additional characterization techniques such as atomic force microscopy, X-ray photoelectron spectroscopy, Raman spectroscopy, and photoluminescence (PL) were used to evaluate the MoS NSs. These studies revealed the high crystallinity and quality of the synthesized NSs. The MoS NSs show visible light emission similar to mechanically exfoliated monolayer MoS NSs. The striking PL signal comes from the exposed edges as shown by experimental and theoretical calculations. The vertical MoS NSs also exhibit a hydrophobic character with a contact angle of 114°. The as-grown MoS NSs would be highly useful in the development of catalysis, nano-optoelectronics, gas-sensing and bio-sensing device applications.