We have investigated the effect of chamber pressure and atmosphere on the microstructure and nanomechanical properties of amorphous carbon thin films prepared by pulsed laser deposition. The amorphous carbon films were deposited in various atmospheres such as nitrogen and argon at different chamber pressures. We used Raman spectroscopy to study the bonding characteristics of the deposited amorphous carbon films. Atomic force microscopy and optical microscopy were utilized to observe the surface conditions and the microstructures of the deposited films. Nanoindentation measurements were carried out on various samples prepared under different conditions to study the effect of chamber pressure and atmosphere on the elastic modulus and nanohardness of the films. It was found that reduced vacuum leads to formation of amorphous carbon films with reduced elastic modulus and nanohardness. Amorphous carbon films prepared under higher chamber pressures exhibit an increased density of particulates and significantly roughened surface. The results were understood in combination with the optical emission and electrostatic measurements of the laser plasma plume. It was found that the presence of atmosphere decreases the leading edge ionic energies of the species in the laser plasma plume and increases the thermalization of the laser plasma due to an increased possibility of collision.