Loneliness is a widely affecting mental health symptom and can be mediated by and co-vary with patterns of social exposure. Using momentary survey and smartphone sensing data collected from 129 Android-using college student participants over three weeks, we (1) investigate and uncover the relations between momentary loneliness experience and companionship type and (2) propose and validate novel geosocial features of smartphone-based Bluetooth and GPS data for predicting loneliness and companionship type in real time. We base our features on intuitions characterizing the quantity and spatiotemporal predictability of an individual's Bluetooth encounters and GPS location clusters to capture personal significance of social exposure scenarios conditional on their temporal distribution and geographic patterns. We examine our features' statistical correlation with momentary loneliness through regression analyses and evaluate their predictive power using a sliding window prediction procedure. Our features achieved significant performance improvement compared to baseline for predicting both momentary loneliness and companionship type, with the effect stronger for the loneliness prediction task. As such we recommend incorporation and further evaluation of our geosocial features proposed in this study in future mental health sensing and context-aware computing applications.