In a recent study, we developed ultralow-binder-content (UBC) structural materials based on lunar soil simulant and thermoset binders. In the current research, we investigated thermoplastic binders. Compared to thermosets, advanced thermoplastics could be more UV resistant, more durable, more robust, and recyclable. Our main technology is the compaction self-assembly (CSA). By using only ~4 wt% polyetherketoneketone (PEKK) binder, the thermoplastic-binder UBC composite was stronger than typical steel-reinforced concrete. The CSA operation was separate from the curing process. This study may provide an important in-situ resource utilization method for large-scale construction on Moon.