Hydrolytic polycondensation of vinyltrimethoxysilane (VTM) was investigated in detail to prepare vinylpolysiloxanes (VPS) having spinnability and tough gel films. VTM was hydrolyzed in various molar ratios r(1) (H2O/VTM) = 0.5-1.6 (HCl/VTM = 0.105, EtOH/VTM = 1.44) at 70 degrees C under a N-2 stream with stirring at 150 rpm to give vinylpolysiloxanes with (Mn) over bar = 510-2100((Mw) over bar/(Mn) over bar = 1.1-10.4). The controlled hydrolysis in r(1) = 1.40-1.64 formed VPSs having the various degrees of spinnability at N2 flow rates of 100-500 ml/min. Transparent films of thickness 0.1-0.05 mm and tensile strength 5-16 MPa were prepared when a 20 wt% acetonemethanol (1: 1, V/V) solution of VPS (r(1) = 1.64) was cast at 80 degrees C for several ten days. The reaction was followed by Si-29-NMR spectroscopy to investigate the distribution of unit structures T-1, T-2 and T-3 in VPS depending on r(1).