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According to IRS publication 501. To claim Head of Household you would need to meet the following qualifications.
You are unmarried or considered unmarried on the last day of the year. ...
If you provided over 85% of your Grandson's support for the year you would be eligible to claim your grandson as a dependent. Of course, if you claim your grandson as a dependent your daughter would not be able to claim him.
I am assuming that you are not married. If this is the case your options would be to file as Head of Household (If you qualify) or single.
It would depend on a few factors. Are the children that you are financially supporting still living with you?
Are they students? Do they earn more than $4,050?