Dysautonomia is a common and severe complication of Guillain-Barré syndrome (GBS), which may manifest as cardiac arrhythmias, labile blood pressure, diaphoresis, and changes in gastrointestinal motility. Takotsubo cardiomyopathy (TCM) is a life-threatening manifestation of dysautonomia in patients with GBS, which is not widely underlined in the literature. The association between GBS and TCM has been well-documented in previous studies; however, there are few reported cases with GBS who developed TCM following their diagnosis with GBS. In this case report, we will discuss our experience treating a 59-year-old female patient who became hemodynamically unstable while recovering from an acute GBS infection. She was diagnosed with TCM after undergoing an echocardiogram and coronary angiogram ruling out thrombotic or obstructive coronary disease and myocarditis.