Despite Large language models' (LLMs) emerging successes, the performance of LLM agents in decision-making has not been fully investigated through quantitative metrics, especially in the multi-agent setting when they interact with each other, a typical scenario in real-world LLM-agent applications. To better understand the limits of LLM agents in these interactive environments, we propose to study their interactions in benchmark decision-making settings in online learning and game theory, through the performance metric of \emph{regret}. We first empirically study the no-regret behaviors of LLMs in canonical (non-stationary) online learning problems, as well as the emergence of equilibria when LLM agents interact through playing repeated games. We then provide some theoretical insights into the no-regret behaviors of LLM agents, under certain assumptions on the supervised pre-training and the rationality model of human decision-makers who generate the data. Notably, we also identify (simple) cases where advanced LLMs such as GPT-4 fail to be no-regret. To promote the no-regret behaviors, we propose a novel \emph{unsupervised} training loss of \emph{regret-loss}, which, in contrast to the supervised pre-training loss, does not require the labels of (optimal) actions. Finally, we establish the \emph{statistical} guarantee of generalization bound for regret-loss minimization, and more importantly, the \emph{optimization} guarantee that minimizing such a loss may \emph{automatically} lead to known no-regret learning algorithms. Our further experiments demonstrate the effectiveness of our regret-loss, especially in addressing the above ``regrettable'' cases.