Can actual instrument time count as simulated instrument time for the PPL?
Provided your CFI and you were flying on a filed and ATC cleared IFR flight plan at the time of the real instrument time was acquired, then yes, you can use that instrument time toward your PPL Aeronautical Experience requirements.  It does not necessarily need to be done under the hood. 61.109(a)(3) just requires the applicant log 3 hours of dual instruction time flying solely on reference to the instruments, whether simulated or real IMC conditions.  

The downside here is that unless you did the dual instrument time with a CFII, you cannot use that time toward an instrument rating or advanced pilot or flight instructor certificates per 61.109.