Hypereutectic Al-high Si alloys are of immense interest for applications in the automotive, space or electronic industries, due their low weight, low thermal expansion, and excellent mechanical and tribological properties. Additionally, their production by laser powder bed fusion (LPBF) technology provides high flexibility in geometrical design and alloy composition. Since, most of the alloy properties could be improved by increasing the Si content, there is much interest in discovering the maximum that could be realized in LBPF Al-high Si alloys, without the appearance of any material failure. For this reason, in this work the production of Al-high Si alloys with extremely high silicon content of up to 70 wt.% was fundamentally investigated with respect to microstructure and mechanical properties. Highly dense (99.3%) and crack-free AlSi50 samples (5 × 5 × 5 mm3), with excellent hardness (225 HV5) and compressive strength (742 MPa), were successfully produced. Further, for the first time, AlSi70 LBPF samples of high density (98.8%) without cracks were demonstrated, using moderate scanning velocities. Simultaneously, the hardness and the compressive strength in the AlSi70 alloys were significantly improved to 350 HV5 and 935 MPa, as a result of the formation of a continuous Si network in the microstructure of the alloy. With respect to the powder source, it was found that the application of powder blends resulted in similar alloy properties as if pre-alloyed powders were used, enabling higher flexibility in prospective application-oriented alloy development.