This dataset is intended for use in conjuction with the publication; On the Effect of Functionalizer Chain Length and Water Content in Polyethylene/Silica Nanocomposites: Part I – Dielectric Properties and Breakdown Strength Authors: I. L. Hosier, M. Praeger, A. F. Holt, A. S. Vaughan and S. G. Swingler which was accepted for publication in IEEE Transactions on Dielectrics and Electrical Insulation on 8th February 2017 Each page of the worksheet corresponds to a seperate figure in the paper Abstract: A series of nanoparticles was prepared by functionalizing a commercial nanosilica with alkylsilanes of varying alkyl tail length, from propyl to octadecyl. By using a constant molar concentration of silane, the density of alkyl groups attached to each system should be comparable. The effect of chain length on the structure of the resulting nanosilica/polyethylene nanocomposites was examined and comparison with an unfilled reference system revealed that, other than through a weak nucleating effect, the inclusion of the nanosilica does not affect the matrix structure. Since water interacts strongly with applied electric fields, water was used as a dielectric probe in conjunction with dielectric spectroscopy to examine the effect of the nanofiller and its surface chemistry on the system. Sets of samples were prepared through equilibrating under ambient conditions, vacuum drying and water immersion. While the water content of the unfilled polymer was not greatly affected, the water content of the nanocomposites varied over a wide range as a result of water accumulation, in a range of states, at nanoparticle interfaces. The effect of water content on breakdown behavior was also explored and, in the unfilled polymer, the breakdown strength was found to depend little on exposure to water (~13% reduction). In all the nanocomposites, the increased propensity for these systems to absorb water meant that the breakdown strength was dramatically affected (>66% reduction).