To develop metal-labeled digoxin radiopharmaceuticals with affinity with anti-digoxin antibody as well as Na+,K(+)-ATPase, a digoxin derivative conjugated with deferoxamine was synthesized. The derivative had a high binding affinity with 67Ga at deferoxamine introduced to the terminal sugar ring of digoxin. The 67Ga labeled digoxin derivative showed enough in vitro binding affinity and selectivity to anti-digoxin antibody as well as Na+,K(+)-ATPase. The 67Ga labeled digoxin derivative is considered to be a potential metal-labeled bifunctional radiopharmaceutical for digoxin RIA as well as myocardial Na+,K(+)-ATPase imaging.