The production of high-performance fiber-reinforced cementitious composites (HPFRCCs) as a durable construction material using different types of fibers and nanomaterials critically relies on the synergic effects of the two materials as well as the cementitious composite mixes. In this study, novel HPFRCCs were developed, which comprised high content (50%) slag by mass of the base binder as well as nano-silica (NS) or nano-crystalline cellulose (NCC). In addition, nano-fibrillated cellulose (NFC), and basalt fiber pellets (BFP), representing nano-/micro- and macro-fibers, respectively, were incorporated into the composites. The response surface method was used in this study’s statistical modeling part to evaluate the impact of key factors (NS, NCC, NFC, BFP) on the performance of 15 mixtures. The composites were assessed in terms of setting times, early- and late-age compressive strength, flexural performance, and resistance to freezing-thawing cycles, and the bulk trends were corroborated by fluid absorption, thermogravimetry, and microscopy tests. Incorporating NS/NCC in the slag-based binders catalyzed the reactivity of cement and slag with time, thus maintaining the setting times within an acceptable range (maximum 9 h), achieving high early- (above 33 MPa at 3 days) and later-age (above 70 MPa at 28 days) strength, and resistance to fluid absorption (less than 2.5%) and frost action (DF above 90%) of the composites. In addition, all nano-modified composites with multi-scale fibers showed notable improvement in terms of post-cracking flexural performance (Residual Strength Index above 40%), which qualify them for multiple infrastructure applications (i.e., shear key bridge joints) requiring a balance between high-strength properties, ductility, and durability.