Population size and density estimates are needed to plan resource requirements and plan health related interventions. Sampling frames are not always available necessitating surveys using non-standard household sampling methods. These surveys are time-consuming, difficult to validate, and their implementation could be optimised. Here, we discuss an example of an optimisation procedure for rapid population estimation using T-Square sampling which has been used recently to estimate population sizes in emergencies. A two-stage process was proposed to optimise the T-Square method wherein the first stage optimises the sample size and the second stage optimises the pathway connecting the sampling points. The proposed procedure yields an optimal solution if the distribution of households is described by a spatially homogeneous Poisson process and can be sub-optimal otherwise. This research provides the first step in exploring how optimisation techniques could be applied to survey designs thereby providing more timely and accurate information for planning interventions.