This work presents the experimental study of hybrid cement-based composites with polyvinyl alcohol fiber (PVA) and alkali-treated, short, natural curaua fiber. The objective of this research is to develop composites reinforced with PVA and curaua fiber to present strain-hardening behavior with average crack width control. To achieve this objective, three groups of composites were investigated. The first group had only PVA fiber in volumes of 0.5, 1, and 2%. The composite with 2% PVA fiber was the only one with strain-hardening and crack width control. The second group had 0.5% PVA fiber and volume fractions of 2, 2.5, and 3% curaua fiber, and presented only deflection-hardening behavior. The third group had 1% PVA and volumes of 1, 1.5, and 2% curaua fiber, and presented strain-hardening behavior. Based on the results, the hybrid combination of 1% PVA and 1.5% curaua was the optimal mixture as it presented strain-hardening behavior and crack width control, with a lower volume of synthetic PVA fiber. Additionally, compressive strength and mix workability were calculated for the investigated composites for comparison.