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Background: The aim of this study was to identify an appropriate screening instrument for the identification of frail elderly patients in a tertiary cancer center. In order to improve cancer care for older patients, the use of a geriatric assessment (GA) has been proposed to identify frail patients or those who are at a higher risk for chemotherapy-related toxicities. In busy clinical routine, an appropriate screening instrument could be used to spare time- and resource-consuming application of GA. Patients and Methods: We administered the Vulnerable Elders Survey (VES-13), G8 questionnaire, and Predictors of Toxicity (POT) as well as a GA at the first visit of 84 consecutive patients at a single Comprehensive Cancer Center. Analysis for patients’ characteristics as well as sensitivity, specificity, and positive and negative predictive value (npv) was conducted. Results: The median age of the patients was 73 years (range 63–93 years), 61.9% were male, most (63%) suffered from gastrointestinal tumors, 39.3% had a multiple cancer diagnosis, and 53.6% had metastasis. 30 (35.7%) individuals were classified as ‘frail’ by the GA. Sensitivity of G8 was 38.3%, and the npv was 63.8%. Sensitivity for VES-13 was 57.1%, and npv was 76.3%. Sensitivity of POT was 72.7%, and the npv was 80.6%. Conclusion: For the first time, the VES13, G8, and POT are compared in a sample of older German patients. The POT seems to be a sufficient screening tool to identify frail patients in a tertiary referral cancer center and helps to save time and resources compared with a complete GA.