While there have been various lost circulation materials (LCMs) available in the market for treating fractures during the drilling of oil and gas wells, there is still a demand for a technology to seal large fractures. Considering limitations on the size of the particles that can be circulated through the drilling equipment, especially the bottomhole assembly, simply enlarging conventional LCM particles becomes ineffective for sealing large vugs and fractures. In this study, we use shape memory polymers (SMPs) to prepare programmed LCMs with various temporary shapes, which can transform to their permanent shapes with much larger dimensions as compared to their temporary shapes. A series of steps for thermomechanical programming of SMP is designed to trigger their expansion at the reservoir temperature. The dimensions of the programmed shapes can be an order of magnitude smaller than the ones for the original shapes, making their transport through the flowlines feasible, and bridging wide-opened fractures possible. The basic idea is that, after recovery, the SMP-based LCMs form an entangled network across a large width of fracture, and SMP particles recovered within the network, filling in the pores to form an effective sealing. We seek the capability of entangled ladders and interwoven fibers in forming a network across the fracture. A permeability plugging apparatus (PPA) is used to examine the efficiency of developed LCMs. The technique of 3D X-ray computed tomography (CT) is used to visualize the internal structure of formed plugs, enabling us to understand the mechanisms of bridging, plugging, and sealing.