Accurate knowledge of the electron density structure of the Earth's upper atmosphere is crucial to forecasting the performance of transionospheric radio signals. For this research, we focus on storm-time structuring in the mid- to high latitude ionosphere where large gradients in electron density can cause severe degradation of communication and navigation signals. We begin in Chapter 2 with a review of the primary data sets and methods used to accomplish the collaborative, multi-instrument studies described in this dissertation. In Chapter 3, we compare observational techniques for tracking polar cap patches during a moderate geomagnetic storm interval. For the first time, we monitor the transportation of patches with high spatial and temporal resolution across the polar cap for 1--2~h using a combination of GPS TEC, all-sky airglow imagers (ASIs), and Super Dual Auroral Radar Network (SuperDARN) HF radar backscatter. Simultaneous measurements from these data sets allow for continuous tracking of patch location, horizontal extent, and velocity even under adverse observational conditions for one or more of the techniques. A focus is placed on the structuring of patches, particularly on the nightside ionosphere as they become wider in the dawn-dusk direction and develop narrow finger-like structures. In Chapter 4, we perform a superposed epoch analysis to characterize the average response of GPS TEC in the North American sector during more than 100 geomagnetic storms over a 13-year interval. For the first time a rigorous approach is used to fully separate storm-time, local time, longitudinal, and seasonal effects at midlatitudes where dense ground receiver coverage is available. The rapid onset of a positive phase is observed across much of the dayside and evening ionosphere followed by a longer-lasting negative phase across all latitudes and local times. Our results show clear seasonal variations in the storm-time TEC, such that summer events tend to be dominated by the negative storm response while winter events exhibit a stronger initial positive phase with minimal negative storm effects. A prominent magnetic declination effect is identified and examined in terms of thermospheric zonal winds pushing plasma upward/downward along magnetic field lines of opposite declination. Finally in Chapter 5 we summarize several co-authored studies which examined various storm-time phenomena utilizing GPS TEC mapping tools developed for this dissertation research, with topics including subauroral polarization stream (SAPS), storm enhanced density (SED), tongue of ionization (TOI), and polar cap patches. / Ph. D.