This paper presents an experimental investigation examining water-cement ratio effects on fiber-matrix interface properties and on matrix fracture properties, which are used for designing mix proportion suitable for achieving strain-hardening behavior at a composite level. A single fiber pullout test and a wedge splitting test were employed to measure the bond properties in a matrix and the fracture toughness of mortar matrix, respectively. Test results showed that the properties tended to increase with decreasing water-cement ratio. Composite design using these test results will be discussed in the follow-up paper.