diff --git a/src/libraries/System.Private.CoreLib/src/System/String.Manipulation.cs b/src/libraries/System.Private.CoreLib/src/System/String.Manipulation.cs
index d208eb3bedf63a..74c0c243d480bc 100644
--- a/src/libraries/System.Private.CoreLib/src/System/String.Manipulation.cs
+++ b/src/libraries/System.Private.CoreLib/src/System/String.Manipulation.cs
@@ -3,6 +3,7 @@
 
 using System.Collections.Generic;
 using System.Diagnostics;
+using System.Diagnostics.CodeAnalysis;
 using System.Globalization;
 using System.Numerics;
 using System.Runtime.InteropServices;
@@ -1846,36 +1847,50 @@ private static void CheckStringSplitOptions(StringSplitOptions options)
 
         // Returns a substring of this string.
         //
-        public string Substring(int startIndex) => Substring(startIndex, Length - startIndex);
-
-        public string Substring(int startIndex, int length)
+        public string Substring(int startIndex)
         {
-            if (startIndex < 0)
+            if (startIndex == 0)
             {
-                throw new ArgumentOutOfRangeException(nameof(startIndex), SR.ArgumentOutOfRange_StartIndex);
+                return this;
             }
 
-            if (startIndex > Length)
+            int thisLength = Length;
+            if (startIndex == thisLength)
             {
-                throw new ArgumentOutOfRangeException(nameof(startIndex), SR.ArgumentOutOfRange_StartIndexLargerThanLength);
+                return string.Empty;
             }
 
-            if (length < 0)
-            {
-                throw new ArgumentOutOfRangeException(nameof(length), SR.ArgumentOutOfRange_NegativeLength);
-            }
+            // Copy Span.Slice checks for perf
+            if ((uint)startIndex > (uint)thisLength)
+                ThrowSubstringArgumentOutRangeException(startIndex, thisLength - startIndex);
 
-            if (startIndex > Length - length)
-            {
-                throw new ArgumentOutOfRangeException(nameof(length), SR.ArgumentOutOfRange_IndexLength);
-            }
+            return InternalSubString(startIndex, thisLength - startIndex);
+        }
+
+        public string Substring(int startIndex, int length)
+        {
+            // Copy Span.Slice checks for perf
+            int thisLength = Length;
+#if TARGET_64BIT
+            // Since start and length are both 32-bit, their sum can be computed across a 64-bit domain
+            // without loss of fidelity. The cast to uint before the cast to ulong ensures that the
+            // extension from 32- to 64-bit is zero-extending rather than sign-extending. The end result
+            // of this is that if either input is negative or if the input sum overflows past Int32.MaxValue,
+            // that information is captured correctly in the comparison against the backing _length field.
+            // We don't use this same mechanism in a 32-bit process due to the overhead of 64-bit arithmetic.
+            if ((ulong)(uint)startIndex + (ulong)(uint)length > (ulong)(uint)thisLength)
+                ThrowSubstringArgumentOutRangeException(startIndex, length);
+#else
+            if ((uint)startIndex > (uint)thisLength || (uint)length > (uint)(thisLength - startIndex))
+                ThrowSubstringArgumentOutRangeException(startIndex, length);
+#endif
 
             if (length == 0)
             {
                 return string.Empty;
             }
 
-            if (startIndex == 0 && length == this.Length)
+            if (length == thisLength)
             {
                 return this;
             }
@@ -1883,6 +1898,26 @@ public string Substring(int startIndex, int length)
             return InternalSubString(startIndex, length);
         }
 
+        [DoesNotReturn]
+        private void ThrowSubstringArgumentOutRangeException(int startIndex, int length)
+        {
+            if (startIndex < 0)
+            {
+                throw new ArgumentOutOfRangeException(nameof(startIndex), SR.ArgumentOutOfRange_StartIndex);
+            }
+            if (startIndex > Length)
+            {
+                throw new ArgumentOutOfRangeException(nameof(startIndex), SR.ArgumentOutOfRange_StartIndexLargerThanLength);
+            }
+            if (length < 0)
+            {
+                throw new ArgumentOutOfRangeException(nameof(length), SR.ArgumentOutOfRange_NegativeLength);
+            }
+            // Check not needed since we only call this when startIndex, length are out of range
+            //if (startIndex > Length - length)
+            throw new ArgumentOutOfRangeException(nameof(length), SR.ArgumentOutOfRange_IndexLength);
+        }
+
         private string InternalSubString(int startIndex, int length)
         {
             Debug.Assert(startIndex >= 0 && startIndex <= this.Length, "StartIndex is out of range!");