This paper presents the outcome of a comprehensive experimental program undertaken to study the performance of cellulose pulp and synthetic PVA (polyvinyl alcohol) based fiber-cement composite under both carbonated and non-carbonated curing conditions at early age. The composites were produced at different rolling pressures (2.5 to 9.0 bar) and subjected to various curing conditions in which the effects of CO2 pressure (1 to 3 bar) and curing time (3 to 9 h) were studied. The mechanical properties (modulus of elasticity (MOE), modulus of rupture (MOR), and toughness), as well as the physical properties (porosity, bulk density, and water absorption), were measured for all samples. Scanning electron microscopy (SEM) was used to investigate the effect of carbonation on porosity change and adhesion of fiber-matrix. A parametric investigation of the effects of the carbonation curing period, CO2 pressure, and rolling pressure on the improvement of the physical and mechanical properties during carbonation curing was performed. Results showed that fiber-cement composites cured with an elevated CO2 pressure of 3 bar, rolling pressure of 3 bar, and 5 h of curing time provided optimal curing conditions resulting in the most desirable mechanical and physical properties. However, toughness was greatly reduced with the increase of the CO2 pressure, curing time, and rolling pressure. Additionally, the carbonation curing improved the bonding between the fiber and the cement matrix because of the precipitation of calcite particularly in the pores of the interfacial transition zone (ITZ) between the cement matrix and the fibers.