The development of hull material with ideal properties to meet all the operation requirements has posed the greatest challenge to flying the airship at high altitude for extended periods. Materials developed in our previous study with a laminated structure achieved high strength-to-weight ratio and excellent gas barrier property at a relatively low total weight. To optimize this novel design and obtain a more comprehensive understanding of the laminate properties, a parametric study involving lamination process parameters (temperature and time), and laminate structural parameter (reinforcement fabric construction), was conducted. The effects of lamination parameters on tensile, peel, tear and helium permeability tests were carried out to assess the laminates. It was found that the tensile strength of the laminate is predominantly determined by the fabric reinforcement material properties. The peel and tear strength results showed that increasing the lamination temperature from 185 °C to 200 °C improved respective strength values. Additionally, the analysis of failure modes and tear propagation suggested that laminate samples with progressive failure have better tear resistant property over those with brutal failure. Extremely low helium permeability was achieved, yet the gas barrier property was not affected by the lamination process parameters and fabric type.