Augmented Reality (AR) and Multimodal Large Language Models (LLMs) are rapidly evolving, providing unprecedented capabilities for human-computer interaction. However, their integration introduces a new attack surface for social engineering. In this paper, we systematically investigate the feasibility of orchestrating AR-driven Social Engineering attacks using Multimodal LLM for the first time, via our proposed SEAR framework, which operates through three key phases: (1) AR-based social context synthesis, which fuses Multimodal inputs (visual, auditory and environmental cues); (2) role-based Multimodal RAG (Retrieval-Augmented Generation), which dynamically retrieves and integrates contextual data while preserving character differentiation; and (3) ReInteract social engineering agents, which execute adaptive multiphase attack strategies through inference interaction loops. To verify SEAR, we conducted an IRB-approved study with 60 participants in three experimental configurations (unassisted, AR+LLM, and full SEAR pipeline) compiling a new dataset of 180 annotated conversations in simulated social scenarios. Our results show that SEAR is highly effective at eliciting high-risk behaviors (e.g., 93.3% of participants susceptible to email phishing). The framework was particularly effective in building trust, with 85% of targets willing to accept an attacker’s call after an interaction. Also, we identified notable limitations such as “occasionally artificial” due to perceived authenticity gaps. This work provides proof-of-concept for AR-LLM driven social engineering attacks and insights for developing defensive countermeasures against next-generation augmented reality threats. The SEAR code and dataset is available at: https://github.com/ 2192537130/searsystem/tree/master.