The data within this depository is divided into four folders (1 -4) which contain connectivity, rheological, FTIR and supplementary data respectively for tested hydrogels. Details of each folder follows: 1_Rheology The folder named: 1_Rheology related data contains a file named: Figure2_Rheology, which contain data associated with Figure 2 in the manuscript 2_FTIR The folder named: 2_FTIR related data contains a file named: Figure3_FTIR, which contain data associated with Figure 3 in the manuscript 3_Connectivity The folder named: 3_Connectivity related data contains a file named: Figure5_connectivity, which contain data associated with Figure 5 in the manuscript 4_Supplementary The folder named: 4_Supplementary related data contains three further folders named FTIR_supp, Rheology_supp and TEM_images. FTIR_supp contains a file relating to the peak fitted curves for the three different compositions (1:2, 1:10 and 1:20) and 30s and 10min relating the Figure S2 in the supplementary information. The file is named: Peak_Fitted_Curves.xls Rheology_supp contains three files relating to the rheological data for a representative sample which relates to FIgure S1 in the supplementary information. These files are named: FigureS1a_1HzAmpSweep.xls, FigureS1b_20HzAmpSweep.xls and FigureS1c_FrequencySweep.xls. TEM_images contains micrographs (in .tif format) at two magnifications (4,000 - low magnification and 12,000x - high magnification) for each different hydrogel samples across each composition (1:2, 1:10 and 1:20) and each vortex duration (30s, 1min, 2min, 5min and 10min). These images related to Figure 4 in the manuscript and Figure S3 in the supplementary information.