While the 3D printing technology for cementitious composites has developed rapidly, a combination of 3DP technology and lightweight engineered cementitious composites (LWECCs) could improve many aspects of the construction industry. In this study, a fibre-reinforced high-performance LWECC for extrusion-based printing was proposed. First, six LWECCs were prepared, incorporating two kinds of hollow glass microspheres (HGMs) in varying replacement ratios of fly ash (FA) at 60 wt%, 80 wt%, and 100 wt%. In addition, polyvinyl alcohol (PVA) fibre was introduced given its shrinkage resistance and improvement in printability performance. Thereafter, fresh property (slump loss and setting time), unconfined compression strength (UCS), and flexural strength experiments thoroughly investigated the optimised LWECC design, which was later calibrated for the printing procedure via a printability assessment, including extrudability and buildability. The UCS, flexural strength, and densities of the printed and cast specimens were compared. Lastly, a microstructural investigation using a scanning electron microscope described the reinforcement mechanism of PVA fibre upon the performance of the printed structures and HGMs. The addition of HGMs significantly improve the lightweight property that reaches a value at 1384 kg/m3 but inevitably negates mechanical properties. The printed LWECC obtains 33.6 MPa for UCS and 9.29 MPa for flexural strength. When the printed filament was perpendicular to loading direction, superior toughness was observed, creating a 63% and 40% increase for UCS and flexural strength, respectively.