Various polyurethane (PU) and hybrid organic-inorganic networks based on isocyanate chemistry were synthesized using a two-stage method. All the networks were amorphous. For PU membranes the morphology and the permeability coefficients of different gases (H-2, N-2, O-2) were a function of the polarity and the chain length of the soft segment and a function of the composition of the networks. The membranes based on the same soft segment chain length and on the same molar composition were structurally nanoheterogeneous systems for the less polar soft segments (alpha,omega-hydroxyterminated hydrogenated polybutadiene and a fatty acid oligoester). They were homogeneous for a polycaprolactone type soft segment. The gas diffusion was appreciably hindered in the case of better miscibility between the soft chains and the hard crosslinks. Decreasing the soft segment length decreased the gas permeability coefficient of the network. As the chemical compositions were changed by increasing the soft segment content, an increase in permeability coefficients was observed. The morphology and transport properties of PU networks and hybrid organic-inorganic networks with low inorganic content were compared for the same soft segment content. The similarities observed between the two types of networks led us to conclude that the organic or inorganic nature of the crosslinking agent has no influence on the gas transport properties of these networks.