It is vital to perform system analysis on integrated biomass gasification in chemical recovery systems in pulp and paper and heat and power plants for polygeneration applications. The proposed integration complements existing pulp and paper and heat and power production systems with production of chemicals such as methane and hydrogen. The potential to introduce gasification-based combined cycles comprising gas turbines and steam turbines to utilize black liquors and wood pellets also merits investigation. To perform such analysis, it is important to first build knowledge on expected synthesis gas composition by gasifying at smaller scale different types of feed stock. In the present paper, the synthesis gas quality from wood pellets gasification has been compared with black liquor gasification by means of numerical simulation as well as through pilot-scale experimental investigations. The experimental results have been correlated into partial least squares models to predict the composition of the synthesis gas produced under different operating conditions. The gas quality prediction models are combined with physical models using a generic open-source modelling language for investigating the dynamic performance of large-scale integrated polygeneration plants. The analysis is further complemented by considering potential gas separation using modern membrane technology for upgrading the synthesis gas with respect to hydrogen content. The experimental data and statistical models presented in this study form an important literature source for future use by the gasification and polygeneration research community on further integrated system analysis.