diff --git a/pandas/core/series.py b/pandas/core/series.py
index 1ea8bbbaa0cfb..22eb33e0a95ed 100644
--- a/pandas/core/series.py
+++ b/pandas/core/series.py
@@ -6718,7 +6718,20 @@ def _binop(self, other: Series, func, level=None, fill_value=None) -> Series:
         this_vals, other_vals = ops.fill_binop(this._values, other._values, fill_value)
 
         with np.errstate(all="ignore"):
-            result = func(this_vals, other_vals)
+            # GH#63250: Use arithmetic_op for arithmetic operations to ensure
+            # consistent behavior with dunder methods (includes _bool_arith_check)
+            # But use direct func call for comparison operations (gt, lt, etc.)
+            if func in (
+                operator.gt,
+                operator.ge,
+                operator.lt,
+                operator.le,
+                operator.eq,
+                operator.ne,
+            ):
+                result = func(this_vals, other_vals)
+            else:
+                result = ops.arithmetic_op(this_vals, other_vals, func)
 
         name = ops.get_op_result_name(self, other)
 
diff --git a/pandas/tests/series/test_arithmetic.py b/pandas/tests/series/test_arithmetic.py
index a77e55612e23d..94d78df665aaf 100644
--- a/pandas/tests/series/test_arithmetic.py
+++ b/pandas/tests/series/test_arithmetic.py
@@ -198,6 +198,20 @@ def test_flex_disallows_dataframe(self):
         with pytest.raises(TypeError, match=msg):
             ser.add(df, axis=0)
 
+    @pytest.mark.parametrize(
+        "opname", ["truediv", "rtruediv", "floordiv", "rfloordiv", "pow", "rpow"]
+    )
+    def test_flex_method_bool_dtype_raises(self, opname):
+        # GH#63250 - flex methods should raise NotImplementedError for bool dtypes
+        # consistent with their dunder counterparts
+        ser = Series([True, False, True])
+        other = Series([False, True, True])
+
+        op = getattr(Series, opname)
+        msg = f"operator '{opname.removeprefix('r')}' not implemented for bool dtypes"
+        with pytest.raises(NotImplementedError, match=msg):
+            op(ser, other)
+
 
 class TestSeriesArithmetic:
     # Some of these may end up in tests/arithmetic, but are not yet sorted