You can use NotContain method:
validationResults.Select(result => result.Tag)
.ToList()
.Should()
.NotContain(ServiceContractRuleKey.MedicalDeclarationNumberRequired);
You can also pass a predicate to NotContain method and simplify your code:
validationResults.Should()
.NotContain(item => item.Tag == ServiceContractRuleKey.MedicalDeclarationNumberRequired);