Agroforestry systems that strategically combine trees and/or shrubs with crops provide ecological and economic benefits. However, barriers including lack of quality tree germplasm, limited access to input and output markets, land tenure insecurity, and inadequate technical knowledge restrict widespread adoption of agroforestry among smallholder farmers. Advances in remote sensing and nanotechnology can help overcome these barriers. Remote sensing through high resolution satellite imagery, light detection and ranging (LiDAR), and aerial photography can map landscapes and provide geospatial information to facilitate agroforestry planning and optimization at farm scales. Nanotechnology involves manipulating matter at nanometer scales and has emerging applications in agriculture. Nanobased tools are emerging for targeted seed and agrichemical delivery, enhanced plant protection, soil remediation, and real-time field-level monitoring. The convergence of nanotechnology with information technology and biotechnology presents new opportunities to enhance agroforestry value chains to benefit smallholders. For example, nanobiosensors integrated with mobile platforms can monitor tree health and translate alerts to remedial actions and services customized to small farm contexts. In spite of significant potential, the use of remote sensing and nanotechnology in agroforestry remains limited and targeted capacity building is needed to promote wider adoption of these innovations in smallholder systems to make agroforestry a viable climate-smart approach to sustaining rural livelihoods.